IDEAS home Printed from https://ideas.repec.org/a/nat/natcom/v15y2024i1d10.1038_s41467-024-50902-z.html
   My bibliography  Save this article

Bridge-rich and loop-less hydrogel networks through suppressed micellization of multiblock polyelectrolytes

Author

Listed:
  • Jihoon Han

    (Pohang University of Science and Technology (POSTECH))

  • Saeed Najafi

    (University of California
    University of California)

  • Youyoung Byun

    (Gwangju Institute of Science and Technology (GIST))

  • Lester Geonzon

    (Kashiwa)

  • Seung-Hwan Oh

    (Hongik University)

  • Jiwon Park

    (Gwangju Institute of Science and Technology (GIST))

  • Jun Mo Koo

    (Chungnam National University)

  • Jehan Kim

    (Pohang University of Science and Technology (POSTECH))

  • Taehun Chung

    (Pohang University of Science and Technology (POSTECH))

  • Im Kyung Han

    (Pohang University of Science and Technology (POSTECH))

  • Suhun Chae

    (Pohang University of Science and Technology (POSTECH))

  • Dong Woo Cho

    (Pohang University of Science and Technology (POSTECH))

  • Jinah Jang

    (Pohang University of Science and Technology (POSTECH))

  • Unyong Jeong

    (Pohang University of Science and Technology (POSTECH))

  • Glenn H. Fredrickson

    (University of California
    University of California)

  • Soo-Hyung Choi

    (Hongik University)

  • Koichi Mayumi

    (Kashiwa
    The University of Tokyo, Kashiwa)

  • Eunji Lee

    (Gwangju Institute of Science and Technology (GIST))

  • Joan-Emma Shea

    (University of California
    University of California)

  • Youn Soo Kim

    (Pohang University of Science and Technology (POSTECH))

Abstract

Most triblock copolymer-based physical hydrogels form three-dimensional networks through micellar packing, and formation of polymer loops represents a topological defect that diminishes hydrogel elasticity. This effect can be mitigated by maximizing the fraction of elastically effective bridges in the hydrogel network. Herein, we report hydrogels constructed by complexing oppositely charged multiblock copolymers designed with a sequence pattern that maximizes the entropic and enthalpic penalty of micellization. These copolymers self-assemble into branched and bridge-rich network units (netmers), instead of forming sparsely interlinked micelles. We find that the storage modulus of the netmer-based hydrogel is 11.5 times higher than that of the micelle-based hydrogel. Complementary coarse grained molecular dynamics simulations reveal that in the netmer-based hydrogels, the numbers of charge-complexed nodes and mechanically reinforcing bridges increase substantially relative to micelle-based hydrogels.

Suggested Citation

  • Jihoon Han & Saeed Najafi & Youyoung Byun & Lester Geonzon & Seung-Hwan Oh & Jiwon Park & Jun Mo Koo & Jehan Kim & Taehun Chung & Im Kyung Han & Suhun Chae & Dong Woo Cho & Jinah Jang & Unyong Jeong &, 2024. "Bridge-rich and loop-less hydrogel networks through suppressed micellization of multiblock polyelectrolytes," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-50902-z
    DOI: 10.1038/s41467-024-50902-z
    as

    Download full text from publisher

    File URL: https://www.nature.com/articles/s41467-024-50902-z
    File Function: Abstract
    Download Restriction: no
    File URL: https://libkey.io/10.1038/s41467-024-50902-z?utm_source=ideas
    LibKey link: if access is restricted and if your library uses this service, LibKey will redirect you to where you can use your library subscription to access this item
    ---><---

    References listed on IDEAS

    as
    1. Zhaoming Zhang & Jun Zhao & Zhewen Guo & Hao Zhang & Hui Pan & Qian Wu & Wei You & Wei Yu & Xuzhou Yan, 2022. "Mechanically interlocked networks cross-linked by a molecular necklace," Nature Communications, Nature, vol. 13(1), pages 1-9, December.
    2. Julien Sautaux & Franziska Marx & Ilja Gunkel & Christoph Weder & Stephen Schrettl, 2022. "Mechanically robust supramolecular polymer co-assemblies," Nature Communications, Nature, vol. 13(1), pages 1-9, December.
    3. Samanvaya Srivastava & Marat Andreev & Adam E. Levi & David J. Goldfeld & Jun Mao & William T. Heller & Vivek M. Prabhu & Juan J. de Pablo & Matthew V. Tirrell, 2017. "Gel phase formation in dilute triblock copolyelectrolyte complexes," Nature Communications, Nature, vol. 8(1), pages 1-9, April.
    4. Chao Lang & Jacob A. LaNasa & Nyalaliska Utomo & Yifan Xu & Melissa J. Nelson & Woochul Song & Michael A. Hickner & Ralph H. Colby & Manish Kumar & Robert J. Hickey, 2019. "Solvent-non-solvent rapid-injection for preparing nanostructured materials from micelles to hydrogels," Nature Communications, Nature, vol. 10(1), pages 1-10, December.
    5. Guillaume Gody & Thomas Maschmeyer & Per B. Zetterlund & Sébastien Perrier, 2013. "Rapid and quantitative one-pot synthesis of sequence-controlled polymers by radical polymerization," Nature Communications, Nature, vol. 4(1), pages 1-9, December.
    Full references (including those not matched with items on IDEAS)

    Most related items

    These are the items that most often cite the same works as this one and are cited by the same works as this one.
    1. Changyong Cai & Shuanggen Wu & Yunfei Zhang & Fenfang Li & Zhijian Tan & Shengyi Dong, 2024. "Bulk transparent supramolecular glass enabled by host–guest molecular recognition," Nature Communications, Nature, vol. 15(1), pages 1-9, December.
    2. Xiaochao Xia & Ryota Suzuki & Tianle Gao & Takuya Isono & Toshifumi Satoh, 2022. "One-step synthesis of sequence-controlled multiblock polymers with up to 11 segments from monomer mixture," Nature Communications, Nature, vol. 13(1), pages 1-11, December.
    3. Xue Yang & Lin Cheng & Zhaoming Zhang & Jun Zhao & Ruixue Bai & Zhewen Guo & Wei Yu & Xuzhou Yan, 2022. "Amplification of integrated microscopic motions of high-density [2]rotaxanes in mechanically interlocked networks," Nature Communications, Nature, vol. 13(1), pages 1-10, December.

    More about this item

    Statistics

    Access and download statistics

    Corrections

    All material on this site has been provided by the respective publishers and authors. You can help correct errors and omissions. When requesting a correction, please mention this item's handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-50902-z. See general information about how to correct material in RePEc.

    If you have authored this item and are not yet registered with RePEc, we encourage you to do it here. This allows to link your profile to this item. It also allows you to accept potential citations to this item that we are uncertain about.

    If CitEc recognized a bibliographic reference but did not link an item in RePEc to it, you can help with this form .

    If you know of missing items citing this one, you can help us creating those links by adding the relevant references in the same way as above, for each refering item. If you are a registered author of this item, you may also want to check the "citations" tab in your RePEc Author Service profile, as there may be some citations waiting for confirmation.

    For technical questions regarding this item, or to correct its authors, title, abstract, bibliographic or download information, contact: Sonal Shukla or Springer Nature Abstracting and Indexing (email available below). General contact details of provider: http://www.nature.com .

    Please note that corrections may take a couple of weeks to filter through the various RePEc services.

    IDEAS is a RePEc service. RePEc uses bibliographic data supplied by the respective publishers.